Achieving high-concentration Cl− ions in non-aqueous electrolytes for high-energy-density Li-Cl2 batteries

Pei LI; Shuo YANG; Jiaxiong ZHU; Shengnan WANG; Yue HOU; Huilin CUI; Ze CHEN; Rong ZHANG; Zhuoxi WU; Yiqiao WANG; Zhiquan WEI; Xinghui LIU; Shaoce ZHANG; Xinliang LI; Chunyi ZHI

doi:10.1016/j.matt.2024.03.010

Achieving high-concentration Cl⁻ ions in non-aqueous electrolytes for high-energy-density Li-Cl₂ batteries

Pei LI, Shuo YANG, Jiaxiong ZHU, Shengnan WANG, Yue HOU, Huilin CUI, Ze CHEN, Rong ZHANG, Zhuoxi WU, Yiqiao WANG, Zhiquan WEI, Xinghui LIU, Shaoce ZHANG, Xinliang LI, Chunyi ZHI

Research output: Journal Publications › Journal Article (refereed) › peer-review

3 Citations (Scopus)

Abstract

Chlorine-based electrochemical energy storage is a promising candidate for sustainable battery technology. The anionic redox reaction of Cl^0/−1 is of interest due to its superior redox potential (1.36 V vs. standard hydrogen electrode [SHE]), capacity (756 mAh g⁻¹), high power, and low cost. Although Cl chemistry has been used in aqueous batteries for a long time, its deployment in organic lithium batteries has been significantly impeded due to the insolubility of Cl⁻ ions (<0.1 M). Scarce oxidizable Cl⁻ blocks redox reactions and the inevitable lithium chloride (LiCl) film passivates electrodes on discharge. We report a eutectic effect to improve the Cl⁻ solubility in organic electrolytes (2 M or higher) by mixing a series of N^-/P-centered chloride salts with lithium bis(trifluoromethanesulfonyl)imide at specific ratios. Based on an optimized Cl⁻ concentration, a Li-Cl² cell using I as a chemical fixation can achieve a three-electron transfer with a specific capacity of 702 mAh g⁻¹ and an energy density of 1,116 Wh kg⁻¹.

Original language	English
Pages (from-to)	1867-1878
Number of pages	12
Journal	Matter
Volume	7
Issue number	5
DOIs	https://doi.org/10.1016/j.matt.2024.03.010
Publication status	Published - 1 May 2024
Externally published	Yes

Bibliographical note

Author contributions: C.Z. conceived the idea and designed the experiments. C.Z. P.L. and X.L. directed the research. X.L. S.Y. J.Z. Y.H. and S.W. conducted the materials characterization and electrochemical measurements. H.C. Z.C. S.Z. Z.W. Y.W. Z.W. and R.Z. assisted with the electrochemical measurements and data analysis. P.L. conducted the DFT calculations. P.L. C.Z. and X.L. co-wrote the manuscript. All authors discussed and analyzed the results.

Publisher Copyright:
© 2024 Elsevier Inc.

Funding

This research was supported by GRF under Project CityU 11304921.

Keywords

eutectic effect
high energy density
high-concentration Cl−
Li-Cl2 batteries
lithium batteries
lithium ion batteries
MAP 5: Improvement

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1016/j.matt.2024.03.010

Cite this

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title = "Achieving high-concentration Cl− ions in non-aqueous electrolytes for high-energy-density Li-Cl2 batteries",

abstract = "Chlorine-based electrochemical energy storage is a promising candidate for sustainable battery technology. The anionic redox reaction of Cl0/−1 is of interest due to its superior redox potential (1.36 V vs. standard hydrogen electrode [SHE]), capacity (756 mAh g−1), high power, and low cost. Although Cl chemistry has been used in aqueous batteries for a long time, its deployment in organic lithium batteries has been significantly impeded due to the insolubility of Cl− ions (<0.1 M). Scarce oxidizable Cl− blocks redox reactions and the inevitable lithium chloride (LiCl) film passivates electrodes on discharge. We report a eutectic effect to improve the Cl− solubility in organic electrolytes (2 M or higher) by mixing a series of N-/P-centered chloride salts with lithium bis(trifluoromethanesulfonyl)imide at specific ratios. Based on an optimized Cl− concentration, a Li-Cl2 cell using I as a chemical fixation can achieve a three-electron transfer with a specific capacity of 702 mAh g−1 and an energy density of 1,116 Wh kg−1.",

keywords = "eutectic effect, high energy density, high-concentration Cl−, Li-Cl2 batteries, lithium batteries, lithium ion batteries, MAP 5: Improvement",

author = "Pei LI and Shuo YANG and Jiaxiong ZHU and Shengnan WANG and Yue HOU and Huilin CUI and Ze CHEN and Rong ZHANG and Zhuoxi WU and Yiqiao WANG and Zhiquan WEI and Xinghui LIU and Shaoce ZHANG and Xinliang LI and Chunyi ZHI",

note = "Author contributions: C.Z. conceived the idea and designed the experiments. C.Z. P.L. and X.L. directed the research. X.L. S.Y. J.Z. Y.H. and S.W. conducted the materials characterization and electrochemical measurements. H.C. Z.C. S.Z. Z.W. Y.W. Z.W. and R.Z. assisted with the electrochemical measurements and data analysis. P.L. conducted the DFT calculations. P.L. C.Z. and X.L. co-wrote the manuscript. All authors discussed and analyzed the results. Publisher Copyright: {\textcopyright} 2024 Elsevier Inc.",

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month = may,

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doi = "10.1016/j.matt.2024.03.010",

language = "English",

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TY - JOUR

T1 - Achieving high-concentration Cl− ions in non-aqueous electrolytes for high-energy-density Li-Cl2 batteries

AU - LI, Pei

AU - YANG, Shuo

AU - ZHU, Jiaxiong

AU - WANG, Shengnan

AU - HOU, Yue

AU - CUI, Huilin

AU - CHEN, Ze

AU - ZHANG, Rong

AU - WU, Zhuoxi

AU - WANG, Yiqiao

AU - WEI, Zhiquan

AU - LIU, Xinghui

AU - ZHANG, Shaoce

AU - LI, Xinliang

AU - ZHI, Chunyi

N1 - Author contributions: C.Z. conceived the idea and designed the experiments. C.Z. P.L. and X.L. directed the research. X.L. S.Y. J.Z. Y.H. and S.W. conducted the materials characterization and electrochemical measurements. H.C. Z.C. S.Z. Z.W. Y.W. Z.W. and R.Z. assisted with the electrochemical measurements and data analysis. P.L. conducted the DFT calculations. P.L. C.Z. and X.L. co-wrote the manuscript. All authors discussed and analyzed the results. Publisher Copyright: © 2024 Elsevier Inc.

PY - 2024/5/1

Y1 - 2024/5/1

N2 - Chlorine-based electrochemical energy storage is a promising candidate for sustainable battery technology. The anionic redox reaction of Cl0/−1 is of interest due to its superior redox potential (1.36 V vs. standard hydrogen electrode [SHE]), capacity (756 mAh g−1), high power, and low cost. Although Cl chemistry has been used in aqueous batteries for a long time, its deployment in organic lithium batteries has been significantly impeded due to the insolubility of Cl− ions (<0.1 M). Scarce oxidizable Cl− blocks redox reactions and the inevitable lithium chloride (LiCl) film passivates electrodes on discharge. We report a eutectic effect to improve the Cl− solubility in organic electrolytes (2 M or higher) by mixing a series of N-/P-centered chloride salts with lithium bis(trifluoromethanesulfonyl)imide at specific ratios. Based on an optimized Cl− concentration, a Li-Cl2 cell using I as a chemical fixation can achieve a three-electron transfer with a specific capacity of 702 mAh g−1 and an energy density of 1,116 Wh kg−1.

AB - Chlorine-based electrochemical energy storage is a promising candidate for sustainable battery technology. The anionic redox reaction of Cl0/−1 is of interest due to its superior redox potential (1.36 V vs. standard hydrogen electrode [SHE]), capacity (756 mAh g−1), high power, and low cost. Although Cl chemistry has been used in aqueous batteries for a long time, its deployment in organic lithium batteries has been significantly impeded due to the insolubility of Cl− ions (<0.1 M). Scarce oxidizable Cl− blocks redox reactions and the inevitable lithium chloride (LiCl) film passivates electrodes on discharge. We report a eutectic effect to improve the Cl− solubility in organic electrolytes (2 M or higher) by mixing a series of N-/P-centered chloride salts with lithium bis(trifluoromethanesulfonyl)imide at specific ratios. Based on an optimized Cl− concentration, a Li-Cl2 cell using I as a chemical fixation can achieve a three-electron transfer with a specific capacity of 702 mAh g−1 and an energy density of 1,116 Wh kg−1.

KW - eutectic effect

KW - high energy density

KW - high-concentration Cl−

KW - Li-Cl2 batteries

KW - lithium batteries

KW - lithium ion batteries

KW - MAP 5: Improvement

UR - http://www.scopus.com/inward/record.url?scp=85191307650&partnerID=8YFLogxK

U2 - 10.1016/j.matt.2024.03.010

DO - 10.1016/j.matt.2024.03.010

M3 - Journal Article (refereed)

AN - SCOPUS:85191307650

SN - 2590-2393

VL - 7

SP - 1867

EP - 1878

JO - Matter

JF - Matter

IS - 5

ER -